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At least 379 records · Page 21

Tropospheric chemistry

The chemistry of the background troposphere, the source region, and the transition regions are discussed. The troposphere is governed by heterogeneous chemistry far more so than the stratosphere. Heterogeneous processes of interest involve scavenging of trace gases by aerosols, cloud and precipitation elements leading to aqueous phase chemical reactions and to temporary and permanent removal of material from the gas phase. Dry deposition is a major removal process for ozone, as well as for other gases of importance in tropospheric photochemistry. These processes are also discussed.

Mohnen, V. A.↗

Lidar measurements from space for tropospheric chemistry investigations: Summary of workshop overview presentation

Over the past decade, NASA has played a lead role in defining the scientific objectives and technology requirements for spaceborne lidar investigations of the atmosphere. An assessment of the potential for conducting lidar measurements from space for investigations that pertain specifically to tropospheric chemistry is presented. A description of potential lidar measurement techniques is given, and the scientific requirements for tropospheric chemistry are reviewed. The current status of airborne lidar measurements of aerosols, O3, and H2O is discussed, and a brief description of the evolution of lidar technology to space is given. Also, the measurement of tropospheric gases with a spaceborne lidar system is evaluated for a wide range of gas species. From this general assessment, it appears feasible to measure aerosols, H2O, O3, NH3, CO, CH4, NO2, atmospheric pressure and temperature, and wind with a lidar from space provided that the appropriate laser and receiver technology is available. For the mid-1990's, it is expected that lidar technology will be available for the measurement of aerosols, H2O, and O3 from a space platform.

Browell, Edward V.↗

Systematic stratospheric-tropospheric exchange viewed from isentropic coordinates

Within the atmosphere's stratification, stratospheric-tropospheric exchange of mass and other properties occurs primarily through quasi-horizontal transport processes within baroclinic wave regimes and through diabatic processes either in the form of deep convection or through systematic meridional variation of incoming and outgoing radiation. These exchange processes include both extrusions of stratospheric air into the troposphere and intrusions of tropospheric air into the stratosphere. The physical processes that govern both meridional and vertical exchange processes within isentropic coordinates are summarized for the global circulation.

Johnson, Donald↗

Tropospheric ozone and aerosol distributions across the Amazon Basin

As a part of the NASA Global Tropospheric Experiment to study the Amazon boundary layer, ozone and aerosol distributions were made measured in July-August 1985 by a NASA Electra aircraft on several long-range flights spanning different areas between Tabatinga and Belem, Brazil. Both positive and negative correlations were found in PBL between aerosol concentrations and O3 mixing ratios. The negative correlations result from the downward transport of relatively clean O3-rich air from the upper troposphere into PBL (which normally has higher aerosol loading and lower O3 concentrations than troposphere); positive correlations are found in biomass-burning plumes, where the aerosols are emitted into the air and O3 is photochemically produced. It was found that, in the dry season, a significant portion of the ozone over the rain forest is a result of biomass burning and that the distribution of photochemically produced O3 is strongly affected by synoptic-scale transport from large fires to the south/southeast.

Browell, E. V.↗

Tropospheric methane from an Amazonian floodplain lake

The sources of methane and its flux to the troposphere from the Amazonian floodplain were investigated during the dry season of July and August 1985, using measurements of methane concentration gradients obtained aboard a houseboat laboratory anchored in Lago Calado, a stratified dendritic lake of about 6-sq km area located near the center of the Amazon Basin. Methane concentrations in the mixed layer of the lake were found to vary from 0.0001 to 0.0055 mM, with no consistent temporal trend. The measured methane flux from the surface of the open lake to the atmosphere averaged 27 mg CH4/sq m per day, consistent with the buildup in ambient methane in the nocturnal surface mixed layer of the troposphere. Ebullition contributed 70 percent to the average total flux. The source of methane to the lake and, ultimately, to the troposphere is the benthic sediments.

Crill, Patrick M.↗

Continuing worldwide increase in tropospheric methane, 1978 to 1987

The average worldwide tropospheric mixing ratio of methane has increased by 11 percent from 1.52 parts per million by volume (ppmv) in January 1978 to 1.684 ppmv in September 1987, for an increment of 0.016 + or - 0.001 ppmv per year. Within the limits of the present measurements, the global tropospheric mixing ratio for methane over the past decade is consistent either with a linear growth rate of 0.016 + or - 0.001 ppmv per year or with a slight lessening of the rate of growth over the past 5 years. No indications were found of an effect of the El Nino-Southern Oscillation-El Chichon events of 1982-83 on total global methane, although severe reductions were reported in the Pacific Northwest during that time period.The growth in tropospheric methane may have increased the water concentration in the stratosphere by as much as 28 percent since the 1940s and 45 percent over the past two centuries and thus could have increased the mass of precipitable water available for the formation of polar stratospheric clouds.

Blake, Donald R.↗

Effect of wet tropospheric path delays on estimation of geodetic baselines in the Gulf of California using the Global Positioning System

Surface Meteorological (SM) and Water Vapor Radiometer (WVR) measurements are used to provide an independent means of calibrating the GPS signal for the wet tropospheric path delay in a study of geodetic baseline measurements in the Gulf of California using GPS in which high tropospheric water vapor content yielded wet path delays in excess of 20 cm at zenith. Residual wet delays at zenith are estimated as constants and as first-order exponentially correlated stochastic processes. Calibration with WVR data is found to yield the best repeatabilities, with improved results possible if combined carrier phase and pseudorange data are used. Although SM measurements can introduce significant errors in baseline solutions if used with a simple atmospheric model and estimation of residual zenith delays as constants, SM calibration and stochastic estimation for residual zenith wet delays may be adequate for precise estimation of GPS baselines. For dry locations, WVRs may not be required to accurately model tropospheric effects on GPS baselines.

Tralli, David M.↗

Tropospheric nitric oxide measurements

Nitric oxide (NO) plays a key role in tropospheric photo-chemistry. The photochemical oxidation of hydrocarbons, for example, can serve as either a source or a sink for ozone, depending on the local abundance of NO. Nitric oxide also helps govern atmospheric concentrations of the hydroxyl (OH) radical. The OH radical is the single most important player in photochemical transformations because it controls the atmospheric lifetimes of so many chemical species. Although NO serves as a very effective catalyst in many important chemical processes, its concentration is low enough to normally be expressed in units of parts per trillion by volume (pptv). Consequently, commercially available detectors for NO (with detection limits of about one part per billion) have proven to be unsuitable for use anywhere except in urban areas and near other local pollution sources. Under the sponsorship of NASA's Global Tropospheric Experiment (GTE), Wallops has developed an extremely sensitive detector with a detection limit of a few pptv. The system was specifically designed for aircraft use, with the objective of applying it in global aircraft studies of tropospheric chemistry. Studies with the detector are examined.

Torres, A. L.↗

Measurements of selected C2-C5 hydrocarbons in the troposphere - Latitudinal, vertical, and temporal variations

The tropospheric distribution of 1077 C2-C5 hydrocarbon samples was determined. Shipboard measurements obtained over the eastern Pacific Ocean reveal large north-to-south gradients for most nonmethane hydrocarbons (NMHCs). The results show that NMHC concentrations can decrease by a factor of two or more during the passage of cold fronts in winter and spring, and that upper tropospheric concentrations were lower than those in the lower troposphere.

Singh, Hanwant B.↗

Use of satellite data and modeling to asses the influence of stratospheric processes on the troposphere

The research is comprised of the following tasks: use of simple analytical and numerical models of a coupled troposphere-stratosphere system to examine the effects of radiation and ozone on planetary wave dynamics and the tropospheric circulation; use of satellite data obtained from the Nimbus 7 Limb Infrared Monitor of the Stratosphere (LIMS) instrument and Solar Backscattered Ultraviolet (SBUV) experiment, in conjunction with National Meteorological Center (NMC) data, to determine the planetary wave vertical structures, dominant wave spectra, ozone spectra, and time variations in diabatic heating rate; and synthesis of the modeling and observational results to provide a better understanding of the effects that stratospheric processes have on tropospheric dynamics.

Nathan, Terrence R.↗

A search for solar related changes in tropospheric weather

The possibility that solar variations associated with the 11-year solar cycle may be the cause of the changes in tropospheric weather and climate has been the subject to scientific investigation for several decades. Meteorologists are greatly concerned with the changes in tropospheric phenomena. An attempt was made to find solar activity related changes in tropospheric weather, by the modulation of the quasi-biennial oscillation (QBO) of zonal wind at 50 mb. Rainfall and surface temperature data for a period of about three solar cycles, 1953 to 1988, from various stations in the Indian subcontinent were utilized. By extension, a possible teleconnection was looked for between the temperature changes in middle atmospheric levels and surface temperature when the data are stratified according to east or west phase of the QBO. The temperature data were averaged for January and February to represent the winter temperature and for July and August to represent the summer temperature.

Mohanakumar, K.↗

Tropospheric ozone in the vicinity of the ozone hole - 1987 Airborne Antarctic Ozone Experiment

Results are presented on ozone measurements in the upper troposphere/lower stratosphere over Antarctica, obtained by NASA DC-8 aircraft during the August/September 1987 Airborne Antarctic Ozone Experiment. The ozone mixing ratios as high as several hundred ppbv were measured, but in all cases these ratios were observed in pockets of upper atmospheric air, both in the vicinity of and away from the location of the ozone hole. The background ozone values in the surrounding troposphere were typically in the range of 20-50 ppbv. Correlation of tropospheric ozone observations with the boundaries of the ozone hole differed in the course of the experiment. During the August 28 - September 2 flights, encounters with ozone-rich air were limited, and the background tropospheric ozone appeared to decrease beneath the hole. For the later flights, and as the ozone hole deepened, the ozone-rich air was frequently observed in the vicinity of the hole, and the average ozone values at the flight altitude were frequently higher than the background values.

Gregory, Gerald L.↗

The China Clipper - Fast advective transport of radon-rich air from the Asian boundary layer to the upper troposphere near California

A series of upper tropospheric radon concentration measurements made over the eastern Pacific and west coast of the U.S. during the summers of 1983 and 1984 has revealed the occurrence of unexpectedly high radon concentrations for 9 of the 61 measurements. A frequency distribution plot of the set of 61 observations shows a distinct bimodal distribution, with approximately 2/5 of the observations falling close to 1 pCi/SCM, and 3/5 falling in a high concentration mode centered at about 11 pCi/SCM. Trajectory and synoptic analyses for two of the flights on which such high radon concentrations were observed indicate that this radon-rich air originated in the Asian boundary layer, ascended in cumulus updrafts, and was carried eastward in the fast moving air on the anticyclonic side of the upper tropospheric jet. The results suggest that the combination of rapid vertical transport from the surface boundary layer to the upper troposphere, followed by rapid horizontal transport eastward represents an efficient mode of long-transport for other, chemically reactive atmospheric trace constituents.

Kritz, Mark A.↗

Distribution of tropospheric ozone determined from satellite data

An analysis of more than 22,000 ozone profiles from Stratospheric Aerosol and Gas Experiment I (SAGE I) (1979-1981) and SAGE II (1984-1987) between 50 deg N and 50 deg S is used in conjunction with 9 years (1979-1987) of daily global depictions of total ozone from the TOMS instrument aboard Nimbus 7 to investigate the spatial distribution and seasonal cycle of the integrated amount of ozone in the troposphere. In the tropics, highest concentrations are found in the eastern Atlantic Ocean downwind (west) of Africa and maximize during the time when biomass burning is most prevalent, between July and October. A different seasonal cycle in the tropics is also observed over Indonesia, where a relative maximum is present in the March-April time frame, likewise consistent with when biomass burning is most prevalent. At mid-latitudes, highest concentrations are found downwind of Asia and maximize in the summer. Relatively higher amounts of tropospheric ozone are similarly observed downwind of North America and Europe. At mid-latitudes, the ratio between the amount of tropospheric ozone in the Northern Hemisphere and the amount in the Southern Hemisphere is 1.4, in good agreement with in situ measurements.

Fishman, Jack↗

Perturbations to tropospheric oxidants, 1985-2035. I - Calculations of ozone and OH in chemically coherent regions

A one-dimensional model based on the sensitivity coefficients of Thompson (1990) is used to calculate regional changes in tropospheric O3 and OH due to specified global or regional changes in CH4 and CO emissions over the period 1985-2035. The methods applied are explained, and the results are presented in extensive tables and graphs and characterized in detail. A 10-15-percent increase in global tropospheric O3 and a 10-15-percent decrease in OH are predicted for both (1) global scenarios with continuing increases in CH4 and CO and (2) regional scenarios where emissions are limited in some regions but not in others; significant regional variation in O3 is predicted for (2). If depletion of O3 in the stratosphere and global warming are introduced into (1) or (2), however, they nearly cancel out the tropospheric O3 increases and OH decreases.

Thompson, Anne M.↗

Model calculations of tropospheric ozone production potential following observed convective events

The profiles of CO, NO, O3, water vapor, and temperature, observed in 1985 during and after a series of convective events over rural areas of the south-central United States, were used to model the nonurban ozone production rates and to evaluate the effects of convective clouds on the tropospheric trace-gas chemistry. A comparison of trace-gas profiles measured in and around a large cumulonimbus during its dissipation showed that ozone production in the upper troposphere may be increased fourfold by convection relative to undisturbed air. The convective enhancement of O3 production for the entire tropospheric comlumn was found to be about 50 percent.

Pickering, Kenneth E.↗

A photochemical model of ozone interference effects in laser detection of tropospheric OH

Laser-generated interference in the laser-induced fluorescence detection of tropospheric hydroxyl is addressed by a detailed photochemical model. This phenomenon arises through photolysis of ozone by the detection laser and subsequent reaction of O(1D) with H2O to form OH. The approach is direct time integration of the coupled differential equations describing the pertinent chemical reactions, collisional energy transfer, and photolytic and spectroscopic processes, including an assessment of limitations due to uncertainties in the input parameters. The goal is to use the model to quantitatively design OH detection methods so that the experimental results need not rely on such a model for interpretation. Previously reported measurements of tropospheric OH appear to have been contaminated by ozone interference effects and by optical saturation of the monitoring transition. However, suggested improvements can reduce the problem to interference levels below 200,000 OH molecules/cu cm, permitting measurements useful for testing theories of fast tropospheric photochemistry.

Smith, Gregory P.↗

Tropospheric ozone and aerosols measured by airborne lidar during the 1988 Arctic boundary layer experiment

Ozone (O3) and aerosol distributions were measured from an aircraft using a differential absorption lidar (DIAL) system as part of the 1988 NASA Global Tropospheric Experiment - Arctic Boundary Layer Experiment (ABLE-3A) to study the sources and sinks of gases and aerosols over the tundra regions of Alaska during the summer. The tropospheric O3 budget over the Arctic was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were usually correlated with descending air from the upper troposphere or lower stratosphere. Several cases of continental polar air masses were examined during the experiment. The aerosol scattering associated with these air masses was very low, and the atmospheric distribution of aerosols was quite homogeneous for those air masses that had been transported over the ice for greater than or = 3 days. The transition in O3 and aerosol distributions from tundra to marine conditions was examined several times. The aerosol data clearly show an abrupt change in aerosol scattering properties within the mixed layer from lower values over the tundra to generally higher values over the water. The distinct differences in the heights of the mixed layers in the two regions was also readily apparent. Several cases of enhanced O3 were observed during ABLE-3 in conjunction with enhanced aerosol scattering in layers in the free atmosphere. Examples are presented of the large scale variations of O3 and aerosols observed with the airborne lidar system from near the surface to above the tropopause over the Arctic during ABLE-3.

Browell, Edward V.↗